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1.
Phys Chem Chem Phys ; 26(18): 13675-13682, 2024 May 08.
Article in English | MEDLINE | ID: mdl-38654606

ABSTRACT

In our preceding paper (Y. Fukui et al., Phys. Chem. Chem. Phys., 2023, 25, 25594-25602), we reported a systematic study of the Ag+-ion conducting behaviour of silver iodide (AgI)-loaded mesoporous aluminas (MPAs) with different pore diameters and AgI-loading ratios. By optimising the control parameters, the Ag+-ion conductivity has reached 7.2 × 10-4 S cm-1 at room temperature, which is more than three orders of magnitude higher than that of bulk AgI. In the present study, the effect of silver bromide (AgBr)-doping in the AgI/MPA composites on Ag+-ion conductivity is systematically investigated for the first time, using variable-temperature powder X-ray diffraction, differential scanning calorimetry, and electrochemical impedance spectroscopy measurements. The AgBr-doped AgI/MPA composites, AgI-AgBr/MPA, formed a homogeneous ß/γ-AgI-structured solid solution (ß/γ-AgIss) for the composites with AgBr ≤ 10 mol%, above which the composites underwent a phase separation into ß/γ-AgIss and face-centred cubic AgBr solid solutions (AgBrss). The onset temperature of the exothermic peaks attributed to the transition from α-AgI-structured solid-solution phase to ß/γ-AgIss or AgBrss decreased with increasing the AgBr-doping ratio. The room-temperature ionic conductivity of the AgI-AgBr/MPA composites exhibited a volcano-type dependence on the AgBr-doping ratio with the highest value (1.6 × 10-3 S cm-1) when the AgBr content was 10 mol%. This value is more than twice as high as that of the highest conducting AgI/MPA found in our previous study.

2.
Phys Chem Chem Phys ; 25(37): 25594-25602, 2023 Sep 27.
Article in English | MEDLINE | ID: mdl-37721053

ABSTRACT

A systematic study of Ag+-ion conducting behavior in Ag+-loaded porous materials was conducted over the entire sub-10 nm region for the first time. The effects of the pore diameter of mesoporous aluminas (MPAs) and the amount of silver iodide (AgI) loaded into MPAs were investigated using N2 gas adsorption/desorption, powder X-ray diffraction, differential scanning calorimetry, and electrochemical impedance spectroscopy measurements. Confinement of AgI in the mesoporous space lowers the phase transition temperature between the ß/γ- and α-phases relative to that of bulk AgI. The AgI-loading into the MPAs with smaller pores led to a more significant decrease in the transition temperature, possibly because the smaller AgI nanoparticles in the pores must have a higher surface energy to stabilize the high-temperature phase. The room-temperature ionic conductivity exhibits a volcano-type dependence on the pore diameter with the highest value when AgI was loaded into MPA with a pore diameter of 7.1 nm (7.2 × 10-4 S cm-1 at room temperature). Concerning the 7.1 nm-MPA, the room-temperature ionic conductivity was the highest for the nearly fully occupied composite, which is more than three orders of magnitude higher than that of the bulk AgI. The present study reveals that the Ag+-ion conductivity in AgI/MPA composites can be controlled by optimizing the pore diameter of MPA and the AgI-loading ratio.

3.
ACS Appl Mater Interfaces ; 11(35): 32084-32089, 2019 Sep 04.
Article in English | MEDLINE | ID: mdl-31429538

ABSTRACT

To enhance the decomposition properties of ethylene, Pt-loaded mesoporous silica (SiO2) was coated onto the scaffolds of cordierite (Mg2Al4Si5O18) membranes (CM) and glass fibers (GF). The surface areas of the mesostructured SiO2 layers coated on CM (CM/meso-SiO2) and GF (GF/meso-SiO2) were, respectively, 118 and 323 times higher than those of the CM and GF. In addition, Pt nanoparticles were homogeneously loaded in the mesopores, which acted as a catalyst. The prepared CM/Pt@meso-SiO2 and GF/Pt@meso-SiO2 showed an efficient and high-performing ethylene decomposition. In particular, the flowers, fruits, and vegetables were well stored with the use of CM/Pt@meso-SiO2 and GF/Pt@meso-SiO2, which effectively decomposed ethylene gas they generated. As a result, Pt@meso-SiO2 with scaffolds (CM and GF) are expected to be effective in commercial application for a practical system of preservation.

4.
Chem Commun (Camb) ; 54(61): 8514-8517, 2018 Jul 26.
Article in English | MEDLINE | ID: mdl-30009299

ABSTRACT

In this work, we fabricate a highly effective catalyst for carbon monoxide oxidation based on gold-loaded mesoporous maghemite nanoflakes which exhibit nearly 100% CO conversion and a very high specific activity of 8.41 molCO gAu-1 h-1 at room temperature. Such excellent catalytic activity is promoted by the synergistic cooperation of their high surface area, large pore volume, and mesoporous structure.

5.
Nanoscale ; 10(10): 4779-4785, 2018 Mar 08.
Article in English | MEDLINE | ID: mdl-29469140

ABSTRACT

Herein, we report the synthesis of gold (Au)-loaded mesoporous iron oxide (Fe2O3) as a catalyst for both CO and NH3 oxidation. The mesoporous Fe2O3 is firstly prepared using polymeric micelles made of an asymmetric triblock copolymer poly(styrene-b-acrylic acid-b-ethylene glycol) (PS-b-PAA-b-PEG). Owing to its unique porous structure and large surface area (87.0 m2 g-1), the as-prepared mesoporous Fe2O3 can be loaded with a considerably higher amount of Au nanoparticles (Au NPs) (7.9 wt%) compared to the commercial Fe2O3 powder (0.8 wt%). Following the Au loading, the mesoporous Fe2O3 structure is still well-retained and Au NPs with varying sizes of 3-10 nm are dispersed throughout the mesoporous support. When evaluated for CO oxidation, the Au-loaded mesoporous Fe2O3 catalyst shows up to 20% higher CO conversion efficiency compared to the commercial Au/Fe2O3 catalyst, especially at lower temperatures (25-150 °C), suggesting the promising potential of this catalyst for low-temperature CO oxidation. Furthermore, the Au-loaded mesoporous Fe2O3 catalyst also displays a higher catalytic activity for NH3 oxidation with a respectable conversion efficiency of 37.4% compared to the commercial Au/Fe2O3 catalyst (15.6%) at 200 °C. The significant enhancement in the catalytic performance of the Au-loaded mesoporous Fe2O3 catalyst for both CO and NH3 oxidation may be attributed to the improved dispersion of the Au NPs and enhanced diffusivity of the reactant molecules due to the presence of mesopores and a higher oxygen activation rate contributed by the increased number of active sites, respectively.

6.
Chem Asian J ; 12(8): 877-881, 2017 Apr 18.
Article in English | MEDLINE | ID: mdl-28371448

ABSTRACT

In the present work, 2.4 nm gold nanoparticles (Au NPs) are uniformly dispersed on mesoporous titania thin films which are structurally tuned by controlling the calcination temperature. The gold content of the catalyst is as high as 27.8 wt %. To our knowledge, such a high loading of Au NPs with good dispersity has not been reported until now. Furthermore, the reaction rate of the gold particles is enhanced by one order of magnitude when supported on mesoporous titania compared to non-porous titania. This significant improvement can be explained by an increase in the diffusivity of the substrate due to the presence of mesopores, the resistance to agglomeration, and improved oxygen activation.

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